首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
Photocatalytic technology offers a practical way to solve the energy crisis by producing hydrogen under sunlight but its performance is encumbered by the fast recombination of photoinduced electron-hole pairs. Constructing heterojunctions to form built-in electric fields could separate these electrons and holes, finally enhancing the photocatalytic efficiency. Herein, a Mn0.5Cd0.5Se/g-C3N4 (MCS/CN) heterojunction was fabricated by a facile method to tap into this advantage. 2%MCS/CN shows a hydrogen evolution rate of up to 354.5 μmol in 3 h, which is 4.49 and 126.6 times that of pure g-C3N4 and Mn0.5Cd0.5Se, respectively. Its photocatalytic stability is proved by six cycling tests. Photocurrent, EIS, along with PL spectra, prove that the recombination of photoinduced electron-hole pairs is inhibited by constructing a heterojunction between Mn0.5Cd0.5Se and g-C3N4. In summary, this work demonstrates the enhancement of photocatalysis by constructing a S-scheme heterojunction and offers a feasible way to develop other effective photocatalysts.  相似文献   

2.
Highly efficient and direct photocatalytic H2 evolution from water via water splitting without using sacrificial reagents is a challenging approach to convert solar energy into renewable and storable chemical energy. Herein, by amalgamating the architecture recommendations and energy band engineering principles into the design formulation, a novel Ag@CoFe2O4/g-C3N4 plasmonic p-n heterojunction photocatalytic system is designed and constructed for the first time. The Ag@CoFe2O4/g-C3N4 photocatalyst so designed, under the illumination of the visible-light (λ > 420 nm), produced H2 and O2 in 2:1 stoichiometric amount at the rates of 335 μmol h?1 and 186 μmol h?1, respectively, with an apparent quantum yield reaching 3.35% at 420 nm, demonstrating that Ag@CoFe2O4 dimer colloids are responsible for oxidation and g-C3N4 for reduction. Moreover, in the presence of triethanolamine, the apparent quantum yield achieved by Ag@CoFe2O4/g-C3N4 is 16.47% with hydrogen produced at the rate 3.5 times higher than the CoFe2O4/g-C3N4 heterojunction photocatalyst with AQY of 5.49%. The combination of Ag plasmonic effect and internal electric field established at the interface of p-type CoFe2O4 and n-type g-C3N4 boosts the separation efficiency of photoexcitons from CoFe2O4 to g-C3N4, extending the visible-light absorption capacity of the systems. The generation of optimum amount of defects like oxygen vacancies at the p-n heterojunction interface due to the structural distortion of CoFe2O4 also plays a prominent photocatalytic enhancement by providing active sites for the adsorption of water molecules for the light driven catalytic reactions. Our work introduces a potential avenue to design efficient photocatalysts by constructing several other suitable p-n heterojunction semiconductor photocatalysts toward practical application in solar energy conversion.  相似文献   

3.
Photocatalytic for water splitting to produce hydrogen is recognized as a low-cost, promising and attractive method to solve environmental problems and energy crises, but finding a high-performance photocatalyst is a big challenge. In this work, we designed a type-II β-AsP/g-C3N4 van der Waals heterostructure as an efficient photocatalyst and had the first principles calculations to analyze its stability, electronic properties, and photocatalytic performance. The results showed that the photocatalyst of β-AsP/g-C3N4 heterostructure met the proper band gap and band edge of the redox potential of water splitting, had effective charge separation of photogenerated electronic holes, and efficient visible light response. Importantly, our research showed that the β-AsP/g-C3N4 heterostructure could proceed spontaneously in thermodynamics and had an excellent photocatalytic performance in further study. It had quite good hydrogen evolution performance with the Gibbs free energy of ?0.02 eV, which is closer to zero than ?0.09 eV of Pt (111). The overpotential of its oxygen evolution reaction is as low as 0.57 V. This work showed excellent development prospects for β-AsP/g-C3N4 heterostructure in the field of photocatalysts, which will promote the development of g–C3N4–based photocatalytic for water splitting.  相似文献   

4.
Mesoporous g-C3N4/Zn–Ti layered double hydroxide (LDH)-laminated van der Waals heterojunction nanosheets were prepared by a facile one-step in situ hydrothermal method. Due to the strong electrostatic interactions between the positively charged Zn–Ti LDH and negatively charged g-C3N4 nanocrystal, a laminated van der Waals heterostructure was successfully formed between Zn–Ti LDH and g-C3N4. The mesoporous g-C3N4/Zn–Ti LDH-laminated van der Waals heterojunction, which had a narrow bandgap of 2.41 eV extended the photoresponse to the visible light region. The obtained heterojunctions showed excellent visible-light-driven photocatalytic performance for the complete removal of ceftriaxone sodium (up to ∼97%) and a high hydrogen production rate (∼161.87 μmol h−1 g−1). This was mainly attributed to the formation of the laminated van der Waals heterojunctions, which favoured charge separation and the absorption of visible light, and the mesoporous structure, which provided more surface active sites. This facile strategy for preparing mesoporous g-C3N4/Zn–Ti LDH-laminated van der Waals heterojunctions offers new insights for the fabrication of high-performance van der Waals heterojunction photocatalytic materials.  相似文献   

5.
Developing high activity and eco-friendly photocatalysts for water splitting is still a challenge in solar energy conversion. In this paper, B doped g-C3N4 quantum dots (BCNQDs) were prepared via a facile molten salt method using melamine and boron oxide as precursors. By introducing BCNQDs onto the surface of g-C3N4, g-C3N4/BCNQDs heterojunction was constructed via hydrothermal treatment. The resulting g-C3N4/BCNQDs heterojunction exhibits enhanced hydrogen evolution performance for water splitting under visible light irradiation. The mechanism underlying the improved photocatalytic activity was explored and discussed based on the formation of heterojunction between g-C3N4 and BCNQDs with well-matched band structure.  相似文献   

6.
Graphite-like carbon nitride (g-C3N4) has attracted great attention for pollutant degradation and clean energy production. The heterojunctions of bismuth halide (BiOX, X = Cl, Br, I) and g-C3N4 are proposed to overcome the shortcomings of the g-C3N4 photocatalyst, such as low charge separation rate and high charge recombination rate. This review paper systematically discusses the progress in synthesis, structure, and applications of heterojunction photocatalytic composites made of g-C3N4 and BiOX based on the understanding of their photocatalytic reaction mechanism. We clarify and summarize structural mechanisms of a single and compound semiconductor to reveal the factors that affect photocatalytic performances. We discuss and compare advantages and disadvantages of versatile preparation processes. Particularly, we focus on the understanding of the structure and characteristics of type II, Z-type, n-n, and p-n heterojunctions and their applications, specifically in pollutant degradation, H2 production by water splitting, CO2 reduction, and medical sterilization. The future prospects of g-C3N4/BiOX composites are also discussed from aspects of their preparation, application, and research methods. This work may offer a good avenue and data reference to develop novel g-C3N4 photocatalytic materials to meet the ever-increasing environmental pollution and energy shortage.  相似文献   

7.
Despite that several strategies have been demonstrated to be effective for improving the catalytic hydrogen evolution activity of bulky g-C3N4, the large-scale hydrogen production over g–C3N4–based photocatalysts still confronts a big challenge. Here, a two-step calcination method is presented in constructing metal oxide/two-dimensional g-C3N4, i.e., Ta2O5/2D g-C3N4 photocatalyst. Thanks to the superiority of the synthetic method, nanostructure engineering forming 2D structure, and surface assembly with another semiconductor, can be realized simultaneously, in which ultrathin structure of 2D g-C3N4 and strong interfacial coupling between two components are two important characteristics. As a result, the structure engineered Ta2O5/2D g-C3N4 induces high photocatalytic hydrogen evolution half reaction rate of ~19,000 μmol g?1 h?1 under visible light irradiation (λ > 400 nm), and an external quantum efficiency (EQE) of 25.18% and 12.48% at 405 nm and 420 nm. The high photocatalytic performance strongly demonstrates the advance of the synchronous engineering of nanostructure and construction of heterostructure with tight interface, both of which are beneficial for the fast charge separation and transfer.  相似文献   

8.
In this work, we researched the effect of PCN-222 (M = Ni, Fe, Co) (PM) with different metal ligands on their photocatalytic performance. Compared with PFe and PCo, PNi has the highest photocatalytic hydrogen evolution efficiency due to the narrowest bandgap and the highest conduction band (CB) position. Furthermore, PCN-222(M)/g-C3N4 (PM/CN) heterojunctions was synthesized by one-pot solvothermal method in which PNi/CN displayed the most outstanding photocatalytic activity for H2 evolution. PNi/CN-1 displayed the highest photocatalytic activity. Its hydrogen evolution rate is 19.3 and 3.7 times higher than that of PNi and CN, respectively. A mechanism is proposed to expound the roles of PNi and the enhancement of visible-light photocatalytic performance of the PNi/CN. This work presents a new perspective for the development of high performance photocatalysts for hydrogen production under visible-light driven.  相似文献   

9.
Excellent light harvest, efficient charge separation and sufficiently exposed surface active sites are crucial for a given photocatalyst to obtain excellent photocatalytic performances. The construction of two-dimensional/two-dimensional (2D/2D) or zero-dimensional/2D (0D/2D) binary heterojunctions is one of the effective ways to address these crucial issues. Herein, a ternary CdSe/WS2/g-C3N4 composite photocatalyst through decorating WS2/g-C3N4 2D/2D nanosheets (NSs) with CdSe quantum dots (QDs) was developed to further increase the light harvest and accelerate the separation and migration of photogenerated electron-hole pairs and thus enhance the solar to hydrogen conversion efficiency. As expected, a remarkably enhanced photocatalytic hydrogen evolution rate of 1.29 mmol g−1 h−1 was obtained for such a specially designed CdSe/WS2/g-C3N4 composite photocatalyst, which was about 3.0, 1.7 and 1.3 times greater than those of the pristine g-C3N4 NSs (0.43 mmol g−1 h−1), WS2/g-C3N4 2D/2D NSs (0.74 mmol g−1 h−1) and CdSe/g-C3N4 0D/2D composites (0.96 mmol g−1 h−1), respectively. The superior photocatalytic performance of the prepared ternary CdSe/WS2/g-C3N4 composite could be mainly attributed to the effective charge separation and migration as well as the suppressed photogenerated charge recombination induced by the constructed type-II/type-II heterojunction at the interfaces between g-C3N4 NSs, CdSe QDs and WS2 NSs. Thus, the developed 0D/2D/2D ternary type-II/type-II heterojunction in this work opens up a new insight in designing novel heterogeneous photocatalysts for highly efficient photocatalytic hydrogen evolution.  相似文献   

10.
In photocatalytic splitting water for hydrogen evolution, narrow light response range and fast electron-hole recombination of g-C3N4 (CN) limit its photocatalytic activity. In this article, the N, S co-doped carbon dots (NSCDs) with up-converted property were loaded on CN nanosheets by thermal polymerization to obtain NSCDs/CN composite catalyst. Characterization, electrochemical researches and hydrogen evolution tests suggest that the photocatalytic activity of CN is greatly promoted by the introduction of NSCDs. Under visible and near-infrared irradiation, the hydrogen evolution rate is 5033.1 μmol g?1 h?1 of NSCDs-5/CN, which is 8.3 times higher than that of CN. The performance improvement is mainly attributed to the increased specific surface area, elevated hydrophilic surface, increased light absorption and suppressed carrier recombination of CN after the introduction of NSCDs. This work unveils the mechanism of the hydrogen evolution activity improvement in NSCDs-5/CN, and also offers a new prospect in the design of high-performance CN-based photocatalysts.  相似文献   

11.
Photocatalytic hydrogen production is considered as an ideal approach to solve global energy crisis and environmental pollution. Graphitic carbon nitride (g-C3N4) has received extensive consideration due to its facile synthesis, stable physicochemical properties, and easy functionalization. However, the pristine g-C3N4 usually shows unsatisfactory photocatalytic activity due to the limited separation efficiency of photogenerated charge carriers. Generally, introducing semiconductors or co-catalysts to construct g–C3N4–based heterojunction photocatalysts is recognized as an effective method to solve this bottleneck. In this review, the advantages and characteristics of various types of g–C3N4–based heterojunction are analyzed. Subsequently, the recent progress of highly efficient g–C3N4–based heterojunction photocatalysts in the field of photocatalytic water splitting is emphatically introduced. Finally, a vision of future perspectives and challenges of g–C3N4–based heterojunction photocatalysts in hydrogen production are presented. Predictably, this timely review will provide valuable reference for the design of efficient heterojunctions towards photocatalytic water splitting and other photoredox reactions.  相似文献   

12.
Urea splitting to produce H2 is as an energy-saving alternative to water electrolysis. However, efficient catalysts are required for the practical implementation of urea splitting because of the high overpotentials of the urea oxidation reaction and the hydrogen evolution reaction. Herein, a Ni-modified direct Z-scheme photocatalyst for the urea oxidation and hydrogen evolution reactions was synthesized by electroplating a WO3/g-C3N4 nanocomposite on Ni-decorated carbon felt (WO/CN–Ni@CF). The 2D/2D nanostructure of the as-synthesized WO3/g-C3N4 composite was confirmed by SEM and TEM. The WO/CN–Ni@CF catalyst electrode exhibited excellent bifunctional photocatalytic activity for the urea oxidation and hydrogen evolution reactions. Consequently, the potential required to generate 100 mA cm?2 in an illuminated photoelectrochemical cell using WO/CN–Ni@CF as the anode and the cathode was reduced from 1.80 to 1.50 V. The photoelectrochemical cell exhibited good stability for 18 h with stable H2 generation.  相似文献   

13.
Graphitic carbon nitride (g-C3N4) is one of the promising two-dimensional metal-free photocatalysts for solar water splitting. Regrettably, the fast electron-hole pair recombination of g-C3N4 reduces their photocatalytic water splitting efficiency. In this work, we have synthesized the CuO/g-C3N4 heterojunction via wet impregnation followed by a calcination method for photocatalytic H2 production. The formation of CuO/g-C3N4 heterojunction was confirmed by XRD, UV–vis and PL studies. Notably, the formation of heterojunction not only improved the optical absorption towards visible region and also enhanced the carrier generation and separation as confirmed by PL and photocurrent studies. The photocatalytic H2 production results revealed that CuO/g-C3N4 photocatalyst demonstrated the increased photocatalytic H2 production rate than bare g-C3N4. The maximum H2 production rate was obtained with 4 wt % CuO loaded g-C3N4 photocatalyst. Importantly, the rate of H2 production was further improved by introducing simple redox couple Co2+/Co3+. Addition of Co2+ during photocatalytic H2 production shuttled the photogenerated holes by a reversible conversion of Co2+ to Co3+ with accomplishing water oxidation. The effective shuttling of photogenerated holes decreased the election-hole pair recombination and thereby enhancing the photocatalytic H2 production rate. It is worth to mention that the addition of Co2+ with 4 wt % CuO/g-C3N4 photocatalyst showed ∼7.5 and ∼2.0 folds enhanced photocatalytic H2 production rate than bare g-C3N4/Co2+ and CuO/g-C3N4 photocatalysts. Thus, we strongly believe that the present simple redox couple mediated charge carrier separation without using noble metals may provide a new idea to reduce the recombination rate.  相似文献   

14.
Engineering surface-active facets of metal cocatalysts is one of the most widely explored strategies to develop advanced photocatalysts and promote photocatalytic solar energy conversion. Here, the surface-active facets of Pd nanocrystals in Pd/g-C3N4 photocatalyst was related to the injection flow rate of PdCl2. When PdCl2 was injected at a low flow rate of 7.5 mL/h (7.5-Pd/g-C3N4), the Pd nanocrystals were uniformly dispersed onto the g-C3N4 with exposed low-index {100} and {111} surface-active facets. However, increasing the injection flow rate to 150 mL/h (150-Pd/g-C3N4) formed Pd nanocrystals where only the {100} surface-active facet was exposed. Under visible light irradiation, the 7.5-Pd/g-C3N4 nanocomposite exhibited excellent water splitting activity for hydrogen production (7.61 mmol g−1 h−1), which was significantly better than with the 150-Pd/g-C3N4 nanocomposite (3.3 mmol g−1 h−1). Theoretical calculations and experimental results confirm the importance of the {111} surface-active facets in the 7.5-Pd/g-C3N4 nanocomposite for promoting photocatalytic activity.  相似文献   

15.
Two-dimensional heterojunction g-C3N4/BCN was constructed via thermal polymerization process. The formed two-dimensional heterostructure could enhance the interfacial contact area between BCN and porous g-C3N4 as well as shorten the photogenerated charge carriers transfer time and distance. The two-dimensional g-C3N4/BCN heterojunction photoanode shows enhanced photoelectrochemical (PEC) performance for water splitting under visible-light irradiation, which primarily originates from the improved charge transfer and separation, and prolonged lifetime of electrons. Under the visible light irradiation, the g-C3N4/BCN heterojunction sample yields a photocurrent density of ∼0.62 mA cm−2 at 1.23 V vs. RHE, which is about eight times as many as that of CN (0.08 mA cm−2) electrode at the same conditions. In addition, the possible electron transfer model and mechanism of PEC water splitting for H2 evolution have been discussed.  相似文献   

16.
Fabricating 0D/2D heterojunctions is considered to be an efficient mean to improve the photocatalytic activity of g-C3N4, whereas their applications are usually restricted by complex preparation process. Here, the 0D/2D SnO2/g-C3N4 heterojunction photocatalyst is prepared by a simple one-step polymerization strategy, in which SnO2 nanodots in-situ grow on the surface of g-C3N4 nanosheets. It shows the outstanding photocatalytic H2 production activity relative to g-C3N4 under the visible light, which is due to the formation of 0D/2D heterojunction significantly contributing to the separation of photogenerated charge carriers. In particular, the H2 production rate over the optimal SnO2/g–C3N4–1 sample is 1389.2 μmol h−1 g−1, which is 6.06 times higher than that of g-C3N4 (230.8 μmol h−1 g−1). Meanwhile, the AQE value of H2 production over the SnO2/g–C3N4–1 sample reaches up to a maximum of 4.5% at 420 nm. This work develops a simple approach to design and fabricate g–C3N4–based 0D/2D heterojunctions for the high-efficiency H2 production from water splitting.  相似文献   

17.
In this work, a novel direct Z-scheme g-C3N5/Zn0.5Cd0.5S (CN/ZCS) heterojunction was successfully synthesized. Furthermore, its photocatalytic activity for hydrogen production was also investigated, whose photoluminescence spectrum revealed the charge transfer procedure of g-C3N5 and ZCS. Moreover, the optimized hydrogen production rate of ZCS with 15 wt% of g-C3N5 (15% CN/ZCS) was about 142.8 mmol/h/g and quantum efficiency (Q.E.) was circa 33.7% under 420 nm monochromatic light. Compared with the pure ZCS and ZCS with 2 wt% of Pt, the 15% CN/ZCS composite exhibited considerable improved hydrogen production rate, which was about 20 times and 7 times, respectively. The formation of CN/ZCS composite resulted in faster separation of the photogenerated electron-hole pairs. Our work may supply valuable data for the application of g-C3N5 on photocatalysis.  相似文献   

18.
Rational design of high-efficiency heterostructure photocatalyst is an effective strategy to realize photocatalytic H2 evolution from pure water, but remains still a considerable challenge. Herein, an anatase/rutile TiO2/g-C3N4 (A/R/CN) multi-heterostructure photocatalyst was prepared by a facile thermoset hybrid method. The combination of two type-II semiconductor heterostructures (i.e., A/R and R/CN) significantly improve the separation and transfer efficiency of photogenerated carriers of anatase TiO2, rutile TiO2 and g-C3N4, and A/R/CN photocatalyst with high activity is obtained. The optimal A/R/CN photocatalyst exhibits significantly increased photocatalytic overall water splitting activity with a rate of H2 evolution of 374.2 μmol g−1h−1, which is about 8 and 4 times that of pure g-C3N4 and P25. Moreover, it is demonstrated to be stable and retained a high activity (ca. 91.2%) after the fourth recycling experiment. This work comes up with an innovative perspective on the construction of multi-heterostructure interfaces to improve the overall photocatalytic water splitting performance.  相似文献   

19.
The photocatalytic hydrogen evolution performance of g-C3N4 was enhanced via the hybridization with montmorillonite (MMT) and using NiCoP as cocatalyst. The highest hydrogen-evolution rate from water splitting under visible-light irradiation observed over MMT/g-C3N4/15%NiCoP was 12.50 mmol g−1 h−1 under 1.0 mmol L−1 of Eosin Y-sensitization at pH of 11, which was ∼26.0 and 1.6 times higher than that of MMT/g-C3N4 (0.48 mmol g−1 h−1) and g-C3N4/15%NiCoP (7.69 mmol g−1 h−1). The apparent quantum yield at 420 nm reached 40.3%. The remarkably improved photocatalytic activity can be ascribed to the increased dispersion of g-C3N4 layers, staggered conduction band potentials between g-C3N4 and NiCoP, as well as the electrostatic repulsion originated from negatively charged MMT. This work demonstrates that MMT can be an outstanding support for the deposition of catalytically active components for photocatalytic hydrogen production.  相似文献   

20.
Construction of heterostructured photocatalysts is a feasible method for improving hydrogen production from water splitting because of its good charge transport efficiency. Herein, we coupled the Ti-MOFs (TiATA) with metal-free graphitic carbon nitride (g-C3N4) to synthesize composites, g-C3N4@TiATA, in which a heterostructure was formed between g-C3N4 and TiATA. The establishment of heterojunctions not only broadens the light absorption range of g-C3N4@TiATA (490 nm) by contrast with g-C3N4 (456 nm), but also greatly accelerates charge migration. Photocatalytic studies present that the construction of heterostructure steering the charges flow from g-C3N4 to TiATA and then delivery to the cocatalyst of Pt nanoparticles, exhibiting an impressively photocatalytic hydrogen production rate (265.8 μmol·h−1) in assistance of 300 W Xenon lamp, which is about 3.4 times as much as g-C3N4/Pt.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号